4.7 Article

Understanding the influence of the composition of the Ag-Pd catalysts on the selective formic acid decomposition and subsequent levulinic acid hydrogenation

Journal

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 45, Issue 35, Pages 17339-17353

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2020.04.180

Keywords

Formic acid; Ag-Pd catalysts; DFT study; Hydrogen transfer; Levulinic acid; Biomass

Funding

  1. SYSPROD project
  2. AXELERA Pole de Competitivite
  3. Campus France
  4. grant SONATA BIS from the National Center of Science (NCN) in Krakow (Poland) [2016/22/E/ST4/00550]

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Formic acid is obtained in equimolar amount with levulinic acid during the hydrolysis of cellulose and thus can be used as a sustainable hydrogen source in the direct levulinic acid hydrogenation towards gamma-valerolactone (biofuel additive). Ag-Pd catalysts prepared by various methods and containing different Ag:Pd ratio were investigated in this context. By combining activity tests, characterization of the main physicochemical properties of the catalysts and DFT study of formic acid decomposition, the key factors responsible for the activity of Ag-Pd catalysts in both the formic acid decomposition and the subsequent hydrogenation of levulinic acid were specified. Pd is shown to be active, but prone to poisoning by CO, while the CO poisoning remains limited on diluted Ag-Pd alloy with strong intermetallic interaction, where its adsorption is very weak thanks to the isolation of Pd atoms. Therefore, the catalyst containing 4%Ag-1%Pd/AlOOH showed the highest selectivity in formic acid decomposition as well as the highest activity in levulinic acid hydrogenation (34% conversion in 5 h at 190 degrees C). (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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